The design and development of intricate artificial architectures have been pursued for decades. Helical covalent polymer (HCP) was recently reported as an unexpected topology that consists of chiral 1D polymers assembled through weak hydrogen bonds from achiral building blocks. However, many questions remained about the formation, driving force, and the single-handedness observed in each crystal. In this work, we reveal a metastable, racemic, fully covalently cross-linked, 3D covalent organic framework (COF) as an intermediate in the early stage of polymerization, which slowly converts into single-handed HCP double helices through partial fragmentation and self-sorting with the aid of a series of hydrogen bonding. Our work provides an intriguing example where weak noncovalent bonds serve as the determining factor of the overall product structure and facilitate the formation of a sophisticated polymeric architecture.

In this work we present the extension of semistochastic heat-bath configuration interaction (SHCI) to work with any two-component and four-component Hamiltonian. The vertical detachment energy (VDE) of AuH2 – and zero-field splitting (ZFS) of NpO2 2+ is calculated by correlating more than 100 spinors in both cases. This work demonstrates the capability of SHCI to treat problems where both relativistic effect and electron correlation are important.